Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China

<p>Water-soluble organic carbon (WSOC) in the cryosphere has an important impact on the biogeochemistry cycling and snow–ice surface energy balance through changes in the surface albedo. This work reports on the chemical characterization of WSOC in 28 representative snowpack samples collected...

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Main Authors: Y. Zhou, C. P. West, A. P. S. Hettiyadura, X. Niu, H. Wen, J. Cui, T. Shi, W. Pu, X. Wang, A. Laskin
Format: Article
Language:English
Published: Copernicus Publications 2021-06-01
Series:Atmospheric Chemistry and Physics
Online Access:https://acp.copernicus.org/articles/21/8531/2021/acp-21-8531-2021.pdf
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language English
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author Y. Zhou
Y. Zhou
C. P. West
A. P. S. Hettiyadura
X. Niu
H. Wen
J. Cui
T. Shi
W. Pu
X. Wang
X. Wang
A. Laskin
A. Laskin
spellingShingle Y. Zhou
Y. Zhou
C. P. West
A. P. S. Hettiyadura
X. Niu
H. Wen
J. Cui
T. Shi
W. Pu
X. Wang
X. Wang
A. Laskin
A. Laskin
Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
Atmospheric Chemistry and Physics
author_facet Y. Zhou
Y. Zhou
C. P. West
A. P. S. Hettiyadura
X. Niu
H. Wen
J. Cui
T. Shi
W. Pu
X. Wang
X. Wang
A. Laskin
A. Laskin
author_sort Y. Zhou
title Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
title_short Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
title_full Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
title_fullStr Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
title_full_unstemmed Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, China
title_sort measurement report: molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern xinjiang, china
publisher Copernicus Publications
series Atmospheric Chemistry and Physics
issn 1680-7316
1680-7324
publishDate 2021-06-01
description <p>Water-soluble organic carbon (WSOC) in the cryosphere has an important impact on the biogeochemistry cycling and snow–ice surface energy balance through changes in the surface albedo. This work reports on the chemical characterization of WSOC in 28 representative snowpack samples collected across a regional area of northern Xinjiang, northwestern China. We employed multimodal analytical chemistry techniques to investigate both bulk and molecular-level composition of WSOC and its optical properties, informing the follow-up radiative forcing (RF) modeling estimates. Based on the geographic differences and proximity of emission sources, the snowpack collection sites were grouped as urban/industrial (U), rural/remote (R), and soil-influenced (S) sites, for which average WSOC total mass loadings were measured as 1968 <span class="inline-formula">±</span> 953 <span class="inline-formula">ng g<sup>−1</sup></span> (U), 885 <span class="inline-formula">±</span> 328 <span class="inline-formula">ng g<sup>−1</sup></span> (R), and 2082 <span class="inline-formula">±</span> 1438 <span class="inline-formula">ng g<sup>−1</sup></span> (S), respectively. The S sites showed the higher mass absorption coefficients at 365 <span class="inline-formula">nm</span> (<span class="inline-formula">MAC<sub>365</sub></span>) of 0.94 <span class="inline-formula">±</span> 0.31 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span> compared to those of U and R sites (0.39 <span class="inline-formula">±</span> 0.11 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span> and 0.38 <span class="inline-formula">±</span> 0.12 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span>, respectively). Bulk composition of WSOC in the snowpack samples and its basic source apportionment was inferred from the excitation–emission matrices and the parallel factor analysis featuring relative contributions of one protein-like (PRLIS) and two humic-like (HULIS-1 and HULIS-2) components with ratios specific to each of the S, U, and R sites. Additionally, a sample from site 120 showed unique pollutant concentrations and spectroscopic features remarkably different from all other U, R, and S samples. Molecular-level characterization of WSOC using high-resolution mass spectrometry (HRMS) provided further insights into chemical differences among four types of samples (U, R, S, and 120). Specifically, many reduced-sulfur-containing species with high degrees of unsaturation and aromaticity were uniquely identified in U samples, suggesting an anthropogenic source. Aliphatic/protein-like species showed the highest contribution in R samples, indicating their biogenic origin. The WSOC components from S samples showed high oxygenation and saturation levels. A few unique CHON and CHONS compounds with high unsaturation degree and molecular weight were detected in the 120 sample, which might be anthraquinone derivatives from plant debris. Modeling of the WSOC-induced RF values showed warming effects of 0.04 to 0.59 <span class="inline-formula">W m<sup>−2</sup></span> among different groups of sites, which contribute up to 16 % of that caused by black carbon (BC), demonstrating the important influences of WSOC on the snow energy budget.</p>
url https://acp.copernicus.org/articles/21/8531/2021/acp-21-8531-2021.pdf
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spelling doaj-c85da90539e246feb43a5279514835992021-06-07T10:14:15ZengCopernicus PublicationsAtmospheric Chemistry and Physics1680-73161680-73242021-06-01218531855510.5194/acp-21-8531-2021Measurement report: Molecular composition, optical properties, and radiative effects of water-soluble organic carbon in snowpack samples from northern Xinjiang, ChinaY. Zhou0Y. Zhou1C. P. West2A. P. S. Hettiyadura3X. Niu4H. Wen5J. Cui6T. Shi7W. Pu8X. Wang9X. Wang10A. Laskin11A. Laskin12Key Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaDepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, USADepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, USADepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, USAKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaKey Laboratory for Semi-Arid Climate Change of the Ministry of Education, College of Atmospheric Sciences, Lanzhou University, Lanzhou 730000, ChinaInstitute of Surface-Earth System Science, Tianjin University, Tianjin 300072, ChinaDepartment of Chemistry, Purdue University, West Lafayette, Indiana 47907, USADepartment of Earth, Atmospheric, and Planetary Sciences, Purdue University, West Lafayette, Indiana 47907, USA<p>Water-soluble organic carbon (WSOC) in the cryosphere has an important impact on the biogeochemistry cycling and snow–ice surface energy balance through changes in the surface albedo. This work reports on the chemical characterization of WSOC in 28 representative snowpack samples collected across a regional area of northern Xinjiang, northwestern China. We employed multimodal analytical chemistry techniques to investigate both bulk and molecular-level composition of WSOC and its optical properties, informing the follow-up radiative forcing (RF) modeling estimates. Based on the geographic differences and proximity of emission sources, the snowpack collection sites were grouped as urban/industrial (U), rural/remote (R), and soil-influenced (S) sites, for which average WSOC total mass loadings were measured as 1968 <span class="inline-formula">±</span> 953 <span class="inline-formula">ng g<sup>−1</sup></span> (U), 885 <span class="inline-formula">±</span> 328 <span class="inline-formula">ng g<sup>−1</sup></span> (R), and 2082 <span class="inline-formula">±</span> 1438 <span class="inline-formula">ng g<sup>−1</sup></span> (S), respectively. The S sites showed the higher mass absorption coefficients at 365 <span class="inline-formula">nm</span> (<span class="inline-formula">MAC<sub>365</sub></span>) of 0.94 <span class="inline-formula">±</span> 0.31 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span> compared to those of U and R sites (0.39 <span class="inline-formula">±</span> 0.11 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span> and 0.38 <span class="inline-formula">±</span> 0.12 <span class="inline-formula">m<sup>2</sup> g<sup>−1</sup></span>, respectively). Bulk composition of WSOC in the snowpack samples and its basic source apportionment was inferred from the excitation–emission matrices and the parallel factor analysis featuring relative contributions of one protein-like (PRLIS) and two humic-like (HULIS-1 and HULIS-2) components with ratios specific to each of the S, U, and R sites. Additionally, a sample from site 120 showed unique pollutant concentrations and spectroscopic features remarkably different from all other U, R, and S samples. Molecular-level characterization of WSOC using high-resolution mass spectrometry (HRMS) provided further insights into chemical differences among four types of samples (U, R, S, and 120). Specifically, many reduced-sulfur-containing species with high degrees of unsaturation and aromaticity were uniquely identified in U samples, suggesting an anthropogenic source. Aliphatic/protein-like species showed the highest contribution in R samples, indicating their biogenic origin. The WSOC components from S samples showed high oxygenation and saturation levels. A few unique CHON and CHONS compounds with high unsaturation degree and molecular weight were detected in the 120 sample, which might be anthraquinone derivatives from plant debris. Modeling of the WSOC-induced RF values showed warming effects of 0.04 to 0.59 <span class="inline-formula">W m<sup>−2</sup></span> among different groups of sites, which contribute up to 16 % of that caused by black carbon (BC), demonstrating the important influences of WSOC on the snow energy budget.</p>https://acp.copernicus.org/articles/21/8531/2021/acp-21-8531-2021.pdf